CN113826248A - Battery current collector including metal plate having through-hole and porous reinforcing material filling through-hole, and secondary battery including the same - Google Patents

Battery current collector including metal plate having through-hole and porous reinforcing material filling through-hole, and secondary battery including the same Download PDF

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Publication number
CN113826248A
CN113826248A CN202080030265.XA CN202080030265A CN113826248A CN 113826248 A CN113826248 A CN 113826248A CN 202080030265 A CN202080030265 A CN 202080030265A CN 113826248 A CN113826248 A CN 113826248A
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current collector
reinforcing material
porous
holes
metal plate
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高约翰
李正鲁
朴钟弼
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LG Corp
LG Energy Solution Ltd
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LG Energy Solution Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/76—Containers for holding the active material, e.g. tubes, capsules
    • H01M4/762—Porous or perforated metallic containers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/80—Porous plates, e.g. sintered carriers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/364—Composites as mixtures
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/664—Ceramic materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/72—Grids
    • H01M4/74—Meshes or woven material; Expanded metal
    • H01M4/742—Meshes or woven material; Expanded metal perforated material
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Composite Materials (AREA)
  • Manufacturing & Machinery (AREA)
  • Ceramic Engineering (AREA)
  • Cell Electrode Carriers And Collectors (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The present invention relates to: a current collector including a metal plate having a plurality of through-holes formed in a thickness direction and a porous reinforcing material filling the through-holes of the metal plate; and a secondary battery including the current collector and providing effects of increasing ionic conductivity of the current collector in a thickness direction and preventing stress from being concentrated at a specific portion.

Description

Battery current collector including metal plate having through-hole and porous reinforcing material filling through-hole, and secondary battery including the same
Technical Field
The present invention relates to a current collector for a battery including a metal plate having through-holes and a porous reinforcing material filling the through-holes, and a secondary battery including the current collector.
This application claims priority from korean patent application No. 10-2019-0127753, filed on 15/10/2019, the entire contents of which are incorporated herein by reference.
Background
As the consumption of fossil fuels leads to an increase in energy prices and concerns about environmental pollution increase, the demand for eco-friendly alternative energy is also increasing. In particular, due to the development of technology and the increase in demand for mobile devices, the demand for secondary batteries as energy sources is rapidly increasing.
As the demand for secondary batteries is diversified and increasing, various types of secondary batteries are being developed. Among them, there is an attempt to increase the ionic conductivity of lithium ions in the thickness direction of a current collector by using a current collector formed with a plurality of through holes. However, the current collector formed with the through-holes has limitations in that the formation of the through-holes causes a reduction in mechanical strength and induces a shape change according to stress concentration. In addition, there is a problem in that gas components generated during deterioration due to the operation of the battery are collected in the through-holes and exist in the form of bubbles, thereby inhibiting ion transport.
Therefore, a new current collector or a secondary battery technology including the same solving the problem is required.
Disclosure of Invention
[ problem ] to
The present invention has been made to solve the above problems, and it is an object of the present invention to provide a current collector for a battery including a metal plate having through-holes and a porous reinforcing material filling the through-holes, and a secondary battery including the current collector.
[ solution ]
In one example, the current collector of the battery of the present invention comprises: a metal plate in which a plurality of through holes are formed in a thickness direction; and a porous reinforcing material filled in the through-holes of the metal plate.
In a specific example, the reinforcing material includes at least one selected from the group consisting of a polymer material, a fiber, an inorganic particle, and a carbon material.
In another specific example, the area fraction in which the through-holes are formed is in the range of 10% to 90%.
In one example, in the battery current collector of the present invention, the porosity of the porous reinforcing material is 10% to 90%, and the air permeability is 100s/100mL to 4000s/100 mL.
In one example, the porous reinforcement has an ionic conductivity of 1X10 at 20 deg.C-10And more than S/cm.
In one example, the porous reinforcing material includes at least one of Polyethylene (PE), polypropylene (PP), polymethyl methacrylate (PMMA), polyvinylidene fluoride (PVdF), carboxymethyl cellulose (CMC), an epoxy resin, and a polyurethane resin.
In one example, the porous reinforcing material has a structure in which fibers having a diameter of 5 to 50 μm and an L/D of 20 or more are dispersed.
In one embodiment, the porous reinforcing material further comprises a lithium salt comprising Li as a cation+And comprises a compound selected from the group consisting of F-、Cl-、Br-、I-、NO3 -、N(CN)2 -、BF4 -、ClO4 -、AlO4 -、AlCl4 -、PF6 -、SbF6 -、AsF6 -、BF2C2O4 -、BC4O8 -、(CF3)2PF4 -、(CF3)3PF3 -、(CF3)4PF2 -、(CF3)5PF-、(CF3)6P-、CF3SO3 -、C4F9SO3 -、CF3CF2SO3 -、(CF3SO2)2N-、(FSO2)2N-、CF3CF2(CF3)2CO-、(CF3SO2)2CH-、CF3(CF2)7SO3 -、CF3CO2 -、CH3CO2 -、SCN-And (CF)3CF2SO2)2N-One or more of the group consisting of as an anion.
In another embodiment, the porous reinforcing material comprises a type of first inorganic particle selected from the group consisting of BaTiO3、Pb(Zr,Ti)O3(PZT)、Pb1-aLaaZr1-bTibO3(PLZT, wherein 0<a<1，0<b<1)、Pb(Mg1/3Nb2/3)O3-PbTiO3(PMN-PT), hafnium oxide (HfO)2)、SrTiO3、SnO2、CeO2、MgO、NiO、CaO、ZnO、ZrO2、Y2O3、Al2O3、TiO2And SiC.
In another specific example, the porous reinforcing material further comprises at least one type of second inorganic particle selected from the group consisting of lithium phosphate (Li)3PO4) Lithium titanium phosphate (Li)cTid(PO4)3，0<d<2，0<d<3) Lithium aluminum titanium phosphate (Li)aAlbTic(PO4)3，0<a<2，0<b<1，0<c<3)、(LiAlTiP)aOb(0<a<4，0<b<13) Lithium lanthanum titanate (Li)aLabTiO3，0<a<2，0<b<3) Lithium germanium thiophosphate (Li)aGebPcSd，0<a<4，0<b<1，0<c<1，0<d<5) Lithium nitride (Li)aNb，0<a<4，0<b<2)、LiaSibSc(0<a<3，0<b<2，0<c<4) And LiaPbSc(0<a<3，0<b<3，0<c<7) Group (d) of (a).
In one example, a porous reinforcement material comprises a porous polymeric substrate and a porous coating layer formed on one or both surfaces of the porous substrate.
In addition, the present invention provides a secondary battery comprising the above battery current collector.
In one example, the secondary battery of the present invention includes an electrode assembly having a structure in which unit cells including a positive electrode, a first separator, and a negative electrode are repeated, and a second separator is located between the unit cells, wherein at least one of the positive electrode and the negative electrode includes: a metal plate in which a plurality of through holes are formed in a thickness direction; and a porous reinforcing material filled in the through-holes of the metal plate.
In a specific example, in each structure of the positive electrode and the negative electrode, the electrode mixture layer is laminated on one surface of the current collector facing the direction of the first separator.
In another specific example, in each of the positive and negative electrodes, the electrode mixture layer is laminated on one surface of the current collector facing the direction of the first separator, and the current collector may include a metal plate formed with a plurality of through-holes in a thickness direction and a porous reinforcing material filled in the through-holes of the metal plate.
[ advantageous effects ]
According to the battery current collector and the secondary battery including the same of the present invention, the ionic conductivity in the thickness direction of the current collector is increased by using the metal plate having a plurality of through-holes in the thickness direction, and the stress concentration is prevented by filling the through-holes with the porous reinforcing material.
According to the current collector for a battery and the secondary battery including the same of the present invention, ion transport within the electrode occurs in both directions of the separator and the current collector, thereby reducing the electrolyte resistance element, and at the same time, the through-hole is filled with a reinforcing material to prevent gas elements generated during the operation of the battery from being located in the through-hole, thereby maintaining the initial performance of the battery for a long time.
Drawings
Fig. 1 to 3 are schematic views each showing a current collector of an embodiment of the present invention.
Fig. 4 is a schematic view illustrating a stack structure of a secondary battery according to an embodiment of the present invention.
Detailed Description
Hereinafter, the present invention will be described in detail with reference to the accompanying drawings. The terms and words used in the present specification and claims should not be construed as being limited to general terms or dictionary terms, and the inventor can appropriately define the concept of terms in order to best describe his invention. The terms and words should be interpreted as meanings and concepts consistent with the technical idea of the present invention.
The present invention provides a battery current collector, comprising: a metal plate having a plurality of through holes formed in a thickness direction; and a porous reinforcing material filled in the through-holes of the metal plate.
In the following examples, the reinforcing material contains at least one selected from the group consisting of a polymer material, a fiber, an inorganic particle, and a carbon material. For example, the reinforcing material may have a structure filled with a porous polymer; a structure in which fibers, inorganic particles, or carbon materials are dispersed in a polymer matrix; or a structure in which fibers, inorganic particles, or carbon materials are dispersed together with a binder.
In the present invention, the metal plate has a plurality of through holes in the thickness direction, and the through holes formed on the metal plate are filled with a polymer composition. In particular, the through-holes are filled with a porous reinforcing material. Thereby, the battery current collector of the present invention can reduce, for example, von Mises stress by reducing the current collector deformation rate corresponding to the applied tension and solving stress concentration. In addition, filling the through-holes formed in the metal plate with a porous reinforcing material has an effect of smoothly moving lithium ions in a direction passing through the current collector.
In one embodiment, in the structure of the through-hole, 10 to 500 holes are formed per unit area of 10cm × 10 cm. Specifically, the number of through holes per unit area may be 10 to 300, 10 to 200, 10 to 100, 10 to 70, 30 to 50, 50 to 500, 100 to 200, 50 to 300, 100 to 500, 30 to 200, or 10 to 200.
In another embodiment, the area fraction in which the through-holes are formed is in a range of 10% to 90%. Specifically, the area fraction of the through-holes formed is in the range of 10% to 90%, 10% to 70%, 10% to 50%, 20% to 90%, 30% to 90%, or 30% to 60%. By controlling the number of through holes per unit area or the area fraction within the above range, the deformation rate of the current collector can be reduced and stress concentration can be prevented without significantly reducing the mechanical strength.
In one embodiment, the porous reinforcing material has a porosity of 10% to 90% and an air permeability of 100s/100mL to 4000s/100 mL. The porous reinforcing material of the present invention has high porosity and excellent air permeability, and thus can achieve high ionic conductivity.
In one embodiment, the porous reinforcement has an ionic conductivity of 1X10 at 20 deg.C-10And more than S/cm. The ionic conductivity of the porous reinforcing material is, for example, 1X10-10To 1X10-7S/cm、1×10-8To 1X10-5S/cm、1×10-6To 1X10-3S/cm、1×10-4To 1X10-2S/cm or 1X10-4To 1X10-1S/cm. In one example, the ionic conductivity of the porous reinforcing material may be calculated by equation 1 below.
[ equation 1]
σ＝t/(Rb*A)
In equation 1, σ is the ionic conductivity (S/cm) of the porous reinforcing material. In addition, t represents the thickness of the porous reinforcing material, Rb represents the bulk resistance of the porous reinforcing material obtained from the impedance spectrum, and a represents the area of the porous reinforcing material.
In one embodiment, the porous reinforcing material comprises at least one of Polyethylene (PE), polypropylene (PP), Polymethylmethacrylate (PMMA), polyvinylidene fluoride (PVdF), carboxymethylcellulose (CMC), epoxy resin, and polyurethane resin. In addition, when the battery current collector of the present invention is applied to an all-solid battery, a solid electrolyte may exist in the through-holes, and at this time, a porous reinforcing material may be mixed with the solid electrolyte and filled in the through-holes.
In another embodiment, the porous reinforcing material has a structure in which fibers having a diameter of 5 to 50 μm and an L/D of 20 or more are dispersed. The structure in which the fibers are dispersed may be a structure in which the fibers are dispersed together with a binder or the fibers are dispersed in a polymer matrix.
In yet another embodiment, the porous reinforcing material may be inorganic particles or carbon materials of various shapes or compositions. The carbon material may be graphene, carbon nanotubes or graphite. For example, the carbon nanotubes are single-walled carbon nanotubes.
In yet another embodiment, the porous reinforcing material comprises a lithium salt. Specifically, the lithium salt contains Li as a cation+. In addition, the lithium salt contains a compound selected from the group consisting of F-、Cl-、Br-、I-、NO3 -、N(CN)2 -、BF4 -、ClO4 -、AlO4 -、AlCl4 -、PF6 -SbF6 -、AsF6 -、BF2C2O4 -、BC4O8 -、(CF3)2PF4 -、(CF3)3PF3 -、(CF3)4PF2 -、(CF3)5PF-、(CF3)6P-、CF3SO3 -、C4F9SO3 -、CF3CF2SO3 -、(CF3SO2)2N-、(FSO2)2N-、CF3CF2(CF3)2CO-、(CF3SO2)2CH-、CF3(CF2)7SO3 -、CF3CO2 -、CH3CO2 -、SCN-And (CF)3CF2SO2)2N-One or more of the group consisting of as an anion. The lithium salt serves as a source of lithium ions in the battery, enabling the lithium battery to function. In the present invention, a lithium salt is eluted from the porous reinforcing material and introduced into the electrolyte solution, thereby increasing the ionic conductivity of the electrolyte solution. When the lithium salt is slowly eluted for a long time or the remaining lithium salt is slowly eluted after the initial elution of a large amount of lithium salt, the lithium salt eluted with the electrolyte may play a role of replenishing the electrolyte consumed in the continuous charge and discharge process.
In yet another embodiment, the porous reinforcing material comprises inorganic particles. In particular, when inorganic particles having a high dielectric constant are used, since it is helpful to increase the degree of dissociation of an electrolyte salt (e.g., lithium salt) in a liquid electrolyte, the ion conductivity of the electrolyte solution can be improved. The kind of these inorganic particles is not particularly limited, and inorganic particles selected from the group consisting of inorganic particles having a dielectric constant of about 5 or more and/or inorganic particles having lithium ion transport ability (in the case of a lithium secondary battery) and mixtures thereof may be used.
The inorganic particles having a dielectric constant of 5 or more may include particles selected from the group consisting of BaTiO3、Pb(Zr,Ti)O3(PZT)、Pb1- aLaaZr1-bTibO3(PLZT, wherein 0<a<1，0<b<1)、Pb(Mg1/3Nb2/3)O3-PbTiO3(PMN-PT), hafnium oxide (HfO)2)、SrTiO3、SnO2、CeO2、MgO、NiO、CaO、ZnO、ZrO2、Y2O3、Al2O3、TiO2And SiC. In the present invention, the inorganic particles having a dielectric constant of 5 or more are also referred to as first inorganic particles.
The inorganic particles having lithium ion transport ability may comprise a material selected from the group consisting of lithium phosphate (Li)3PO4) Lithium titanium phosphate (Li)cTid(PO4)3，0<d<2，0<d<3) Lithium aluminum titanium phosphate (Li)aAlbTic(PO4)3，0<a<2，0<b<1，0<c<3)、(LiAlTiP)aOb(0<a<4，0<b<13) Lithium lanthanum titanate (Li)aLabTiO3，0<a<2，0<b<3) Lithium germanium thiophosphate (Li)aGebPcSd，0<a<4，0<b<1，0<c<1，0<d<5) Lithium nitride (Li)aNb，0<a<4，0<b<2)、LiaSibSc(0<a<3，0<b<2，0<c<4) And LiaPbSc(0<a<3，0<b<3，0<c<7) At least one of the group consisting of. In the present invention, the inorganic particles having lithium ion transport ability are also referred to as second inorganic particles.
In the present invention, any of the first and second inorganic particles may be used alone or as a mixture. When the first and second inorganic particles are used in combination, the content ratio of the first and second inorganic particles is 20 to 60:40 to 80, or 40 to 60:40 to 60 on the basis of the weight ratio.
The inorganic particles are dispersed in a polymer matrix that forms the porous reinforcement material. For example, the polymer film may include a porous structure formed due to interstitial volumes between the inorganic particles.
In particular embodiments of the invention, the inorganic particles have a size of 10nm to 20 μm, 100nm to 3.5 μm, or 300nm to 900 nm. It is preferable that the inorganic particles have a uniform size and small variations. Non-uniform particle size can cause the thickness of the polymer film to become non-uniform. In addition, the smaller the particle diameter, the larger the surface area of the particles, and thus the content of the binder resin to be used may be increased and the dispersibility may be reduced. On the other hand, the increase in particle size may cause the film thickness to become excessively thick.
In the present invention, the lithium salt and the inorganic particles may have a structure contained in the porous reinforcing material or dispersed on the surface of the porous reinforcing material. Alternatively, the porous reinforcing material may have a structure including a polymer substrate and a porous coating layer coated on one or both sides of the polymer substrate. In this case, the lithium salt and the inorganic particles are dispersed in the polymer base material, and at the same time, may also be used as a component for forming the porous coating layer.
When both the lithium salt and the inorganic particles are contained, the content ratio of the lithium salt and the inorganic particles is 10 to 40:60 to 90, or 20 to 40:80 to 60 on the basis of the weight ratio. When the content of the lithium salt is too small, the amount of eluted lithium ions is small, and the amount of pores generated by the elution of the lithium salt is insufficient, so that it is difficult to achieve a desired level of ionic conductivity. On the other hand, if the amount of the lithium salt exceeds the above range and is added in a large amount, heat resistance may be deteriorated due to the addition of a small amount of inorganic particles or binder resin, mechanical properties may be deteriorated due to excessive pore formation due to elution of the lithium salt, and metallic lithium may be precipitated at the interface due to the decrease in adhesion between the current collector and the electrode mixture layer. In addition, in the case where the content of the inorganic particles is too small, the interstitial volume between the particles is reduced, and a binder resin is added to form a predetermined thickness, thereby reducing the porosity of the porous coating layer; in the case where the inorganic particles are added in excess of the above range, the packing density may increase during slurry coating and drying, thereby decreasing the air permeability.
In another embodiment, when the coating layer including the lithium salt and/or the inorganic particles is formed, the coating layer may further include a binder component. For example, the coating layer contains inorganic particles, lithium salt, and a binder resin, and the inorganic particles are connected and fixed to each other by the binder resin to form a porous structure.
In one embodiment, the porous reinforcing material comprises a porous polymeric substrate and a porous coating layer formed on one or both surfaces of the porous substrate. The polymer base material may have a structure in which pores are formed during polymerization or a structure in which pores are formed by stretching. In addition, the porous coating layer may have a structure in which inorganic particles are coated on the surface of the polymer substrate. The inorganic particle coating serves to increase the ionic conductivity without inhibiting the porosity of the polymeric substrate.
For example, the porous polymer substrate is formed of a polyolefin resin, and the porous coating layer contains inorganic particles, a lithium salt, and a binder resin, and the inorganic particles are connected and fixed to each other by the binder resin to form a porous structure. Specifically, the porous polymer substrate is a thin film in the form of a sheet, which can be applied if it has excellent ion permeability and mechanical strength. The material of such a polymer substrate may include a polyolefin-based film (e.g., polypropylene) having excellent chemical resistance, and a sheet or nonwoven fabric made of glass fiber or polyolefin, etc. As commercially available products, for example, Celgard TM2400,2300 (manufactured by Hoechest Celanese corp), polypropylene film (manufactured by Ube Industrial Ltd. or Pall RAI) or polyethylene (Tonen or Entek) group products can be used, but not limited thereto. In addition, the porous coating layer serves to supplement the mechanical strength of the porous reinforcing material and impart heat resistance.
The inorganic particles are connected and fixed to each other by a binder resin described below to form a porous structure. The porous coating layer has a porous structure formed by interstitial volumes between the inorganic particles, the interstitial volumes being spaces defined by the inorganic particles substantially in surface contact in a close-packed structure or a close-packed structure.
The binder resin is not particularly limited as long as it exhibits a binding force with the electrode mixture layer stacked on the current collector and a binding force between the inorganic component and the lithium salt in the mixed coating layer and is not easily dissolved by the electrolyte solution. For example, the binder resin may be selected from the group consisting of polyvinylidene fluoride (PVdF), polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-trichloroethylene, polyvinylidene fluoride-chlorotrifluoroethylene (PVdF-CTFE), polymethyl methacrylate, polyacrylonitrile, polyvinylpyrrolidone, polyvinyl acetate, ethylene-vinyl acetate copolymer (polyethylene-co-vinyl acetate), polyethylene oxide, cellulose acetate, cellulose acetate butyrate, cellulose acetate propionate, cyanoethyl pullulan, cyanoethyl polyvinyl alcohol, cyanoethyl cellulose, cyanoethyl sucrose, pullulan, carboxymethyl cellulose, acrylonitrile-styrene-butadiene copolymer, and polyimide, and may specifically be PVdF or PVdF-CTFE.
In consideration of the bonding strength between the inorganic particles and/or the lithium salt and the bonding strength between the current collector and the electrode mixture, the content of the binder resin may be 0.1 to 20 wt%, or 1 to 10 wt% in 100 wt% of the porous coating layer.
In addition, the present invention provides a secondary battery including the above battery current collector.
In one embodiment, the secondary battery of the present invention includes an electrode assembly having a structure in which unit cells including a positive electrode, a first separator, and a negative electrode are repeated, and a second separator is located between the unit cells. Any one or more of the positive electrode and the negative electrode may include a metal plate having a through-hole in a thickness direction and an ion-conductive porous reinforcing material filled in the through-hole of the metal plate.
In one embodiment, the ionic conductivity of the porous reinforcement material at 20 ℃ is 1x10 according to equation 1-4The above.
In another embodiment, in each of the structures of the positive electrode and the negative electrode, the electrode mixture layer is laminated on one surface of the current collector facing the direction of the first separator.
In a specific embodiment, in each of the structures of the positive electrode and the negative electrode, the electrode mixture layer is laminated on one surface of the current collector facing a direction of the first separator, and the current collector may include: a metal plate having a through hole in a thickness direction; and an ion-conductive porous reinforcing material filled in the through-holes of the metal plate.
The secondary battery in the present invention is, for example, a lithium secondary battery. The lithium secondary battery may include, for example: the above electrode assembly; impregnating a non-aqueous electrolyte of the electrode assembly; and a battery case including the electrode assembly and the non-aqueous electrolyte.
The positive electrode has a structure in which a positive electrode mixture layer is stacked on one side or both sides of a positive electrode current collector. These positive electrode active materials may each independently be a lithium-containing oxide, and may be the same or different. A lithium-containing transition metal oxide may be used as the lithium-containing oxide. In one example, the positive electrode mixture layer includes a conductive material and a binder polymer in addition to the positive electrode active material, and may further include a positive electrode additive commonly used in the art, if necessary.
The current collector for the positive electrode is a metal having high electrical conductivity, and any metal that can easily adhere to the positive electrode active material slurry and has no reactivity in the voltage range of the electrochemical device may be used. Specifically, non-limiting examples of current collectors for positive electrodes include aluminum, nickel, or foils made from combinations thereof. Specifically, the current collector for the positive electrode is formed of the above-described metal composition, and includes a metal plate having through-holes in the thickness direction and an ion-conductive porous reinforcing material filled in the through-holes of the metal plate.
The negative electrode may further include a negative electrode mixture layer, and may include a carbon material, lithium metal, silicon, or tin. When a carbon material is used as the anode active material, both low-crystalline carbon and high-crystalline carbon may be used. Representative examples of the low crystalline carbon include soft carbon and hard carbon. Representative examples of highly crystalline carbon include natural graphite, kish graphite, pyrolytic carbon, mesophase pitch-based carbon fibers, medium carbon microspheres, mesophase pitch, and high temperature calcined carbon, such as petroleum or coal pitch derived coke.
Non-limiting examples of current collectors for the negative electrode include copper, gold, nickel, or foil made of copper alloy, or combinations thereof. In addition, the current collector may be used by stacking substrates made of the above-described materials. Specifically, the current collector for the negative electrode is formed of the above-described metal composition, and includes a metal plate having through-holes in the thickness direction and an ion-conductive porous reinforcing material filled in the through-holes of the metal plate.
In addition, the negative electrode may include a conductive material and a binder commonly used in the art.
The first and second separators may be made of any porous substrate used in a lithium secondary battery, for example, a polyolefin-based porous film or a nonwoven fabric may be used, but the present invention is not particularly limited thereto. Examples of the polyolefin-based porous film include films of polyethylene such as high-density polyethylene, linear low-density polyethylene, ultrahigh-molecular-weight polyethylene, and polyolefin-based polymers (e.g., polypropylene, polybutene, and polypentene) each formed alone or in a mixture thereof.
According to an embodiment of the present invention, the electrolyte may be a non-aqueous electrolyte. Examples of the solvent of the non-aqueous electrolyte include N-methyl-2-pyrrolidone, propylene carbonate, ethylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, γ -butyrolactone, 1, 2-dimethoxyethane, tetrahydrofuran, 2-methyltetrahydrofuran, dimethylsulfoxide, 1, 3-dioxolane, formamide, dimethylformamide, dioxolane, acetonitrile, nitromethane, methyl formate, methyl acetate, phosphoric acid triester, trimethoxymethane, dioxolane derivatives, sulfolane, methylsulfolane, 1, 3-dimethyl-2-imidazolidinone, propylene carbonate derivatives, tetrahydrofuran derivatives, ether, methyl pyrophosphate, ethyl propionate and the like. However, the electrolyte is not particularly limited thereto, and various electrolyte components commonly used in the field of lithium secondary batteries may be added or deleted within an appropriate range.
Hereinafter, the present invention will be described in more detail by way of examples and drawings.
Example 1: manufacture of current collectors
A plurality of through-holes of full thickness are formed in the aluminum foil. A solution obtained by mixing a polyethylene resin, a Methyl Ethyl Ketone (MEK) solvent, and a polyvinylidene fluoride (PVdF) binder in an amount of 100:30:5 parts by weight was coated on the surface using a first blade, at which time the solution filled the through-holes, and the residue formed a coating on the foil surface. At this point, the remaining coating on the foil surface is wiped off using a second doctor blade. When the remaining coating layer is not sufficiently removed depending on viscosity and volatility according to the type and composition of the coating solution, the remaining coating layer is removed by the third polishing.
The resulting current collector is shown in fig. 1. Referring to fig. 1, the current collector has a structure in which a plurality of through-type holes are formed in a metal plate 110 made of aluminum foil having a width of 10cm and a length of 10 cm. The through-type pores of the metal plate 110 are filled with the porous reinforcing material 120. The porous reinforcing material 120 is formed of polyethylene resin.
Example 2: manufacture of current collectors
A current collector was manufactured in the same manner as in example 1, except that a polypropylene resin was used instead of the polyethylene resin.
The resulting current collector is shown in fig. 2. Referring to fig. 2, the current collector has a structure in which a plurality of through-type holes are formed in a metal plate 210 made of aluminum foil having a width of 10cm and a length of 10 cm. The through-type holes of the metal plate 210 are filled with a porous reinforcing material 220. The porous reinforcing material 220 is formed of polypropylene resin.
Example 3: manufacture of current collectors
A plurality of through-holes of full thickness are formed in the aluminum foil. A solution of 100:30 parts by weight of polypropylene short fibers and Methyl Ethyl Ketone (MEK) solvent was filled in the through-type holes of the aluminum foil. Then, it was rolled and dried. The diameter of the staple fibers was 20 μm and the L/D was about 50.
Example 4: manufacture of current collectors
A current collector was manufactured in the same manner as in example 1, except that a copper foil was used instead of the aluminum foil.
The resulting current collector is shown in fig. 3. Referring to fig. 3, the current collector has a structure in which a plurality of through holes are formed in a metal plate 310 made of copper foil having a width of 10cm and a length of 10 cm. The through-type holes of the metal plate 310 are filled with a porous reinforcing material 320. The porous reinforcing material 320 is formed of polyethylene resin.
Comparative example 1: manufacture of current collectors
A plurality of through-holes of full thickness are formed in the aluminum foil.
Example 5: manufacture of secondary battery
100 parts by weight of NCM (LiNi) as a positive electrode active material0.8Co0.1Mn0.1O2) 1.5 parts by weight of carbon black (FX35, Denka) as a conductive material and 2.3 parts by weight of polyvinylidene fluoride (KF9700, Kureha) as a binder polymer were added to NMP (N-methyl-2-pyrrolidone) as a solvent, thereby preparing a positive electrode mixture layer slurry. The slurry of the positive electrode mixture layer was poured at 640mg/25cm2The supported amount of (b) was coated on one side of the current collector of example 1, and then vacuum-dried, thereby obtaining a positive electrode.
100 parts by weight of artificial graphite (GT, Zichen (china)), 1.1 parts by weight of carbon black (Super-P), 2.2 parts by weight of styrene-butadiene rubber, and 0.7 part by weight of carboxymethyl cellulose as a conductive material were added to water as a solvent to prepare a negative active material, which was then coated, dried, and pressed on one side of the current collector of example 4, thereby manufacturing a negative electrode.
On the other hand, polypropylene was uniaxially stretched using a dry process to prepare a separator having a microporous structure with a melting point of 165 ℃ and a one-side width of 200 mm. Preparing an electrode assembly having a structure in which: the first separator is located between the positive electrode and the negative electrode, and the second separator is located outside the positive electrode and the negative electrode. The electrode assembly was then mounted in a battery case, and a 1M LiPF6 carbonate electrolyte solution was injected, thereby completing the battery.
A cross-sectional structure of an electrode assembly included in the manufactured secondary battery is shown in fig. 4. Referring to fig. 4, the electrode assembly 400 of the present invention has a structure in which unit cells including positive electrodes 410 and 411, a first separator 431, and negative electrodes 420 and 421 are repeated, and a second separator 432 is located between the unit cells.
Experimental example 1 ion conductivity measurement
The ionic conductivity of the porous reinforcing material filled in the pores of the current collector of example 1 was measured. After gold (Au) electrodes were coated on top of the porous reinforcing material filled in the pores of the current collector prepared in example 1 in a circle having a diameter of 1mm using a sputtering method, ionic conductivity was measured according to temperature using an alternating current impedance measurement method. The ionic conductivity was measured using a VMP3 measuring device and 4294A in the frequency range of 100MHz to 0.1 Hz.
As a result of the measurement, it was confirmed that the ionic conductivity of the porous reinforcing material filled in the pores of the current collector of example 1 was about 1.0x10-3 S/cm。
Experimental example 2 evaluation of Current collector Performance
Various magnitudes of tensile force were applied to the current collectors prepared in comparative example 1, and the resulting length deformation and von Mises stress were evaluated. The results are shown in table 1 below.
In the case of aluminum, a Young's modulus of 70GPa is used. Polypropylene (PP) is a reinforcing material that can be filled in the pores and has a young's modulus of 1.5Gpa to 2 Gpa. In addition, reinforced polymers, such as glass reinforced polyester matrices (17.2GPa), may be used. In this experimental example, a reinforced polymer having a young's modulus adjusted to 5.0Gpa was used as a reinforcing material.
[ Table 1]
F _ tension (MPa) Porosity of the material Displacement field, X component (m) Total displacement (m) Von Mises stress (GPa)
500 0.3217 7.68E-06 7.78E-06 0.78199
1,000 0.3217 1.54E-05 1.56E-05 1.564
1,500 0.3217 2.30E-05 2.33E-05 2.346
Various amounts of tension were applied to the current collectors prepared in example 1, and the resulting length deformation and von Mises stress were evaluated. The results are shown in table 2 below.
[ Table 2]
F _ tension (MPa) Porosity of the material Displacement field, X component (m) Total displacement (m) Von Mises stress (GPa)
500 0.3217 6.70E-06 6.81E-06 0.51205
1,000 0.3217 1.34E-05 1.36E-05 1.0241
1,500 0.3217 2.01E-05 2.04E-05 1.5362
The physical property evaluation results of the current collectors prepared in comparative example 1 and example 1 were compared. Specifically, the difference between the physical property value of the sample of example 1 and the physical property value of the sample of comparative example 1 was converted into a percentage value. The results are shown in table 3 below.
[ Table 3]
x shift change (%) Total shift change (%) von Mises stress Change (%)
6.70E-06 6.81E-06 0.51205
1.34E-05 1.36E-05 1.0241
2.01E-05 2.04E-05 1.5362
Referring to table 3, when comparing the deformed length when the tension is applied, the deformed length of the sample of example 1 is reduced by about 10% compared to the deformed length of the sample of comparative example 1. Furthermore, when comparing von Mises stress, the von Mises stress of the sample of example 1 was reduced by about 35% compared to the von Mises stress of the sample of comparative example 1. The invention has been described in more detail above by means of figures and examples. However, the embodiments described in the specification and the configurations described in the drawings are only the most preferable embodiments of the present invention, and do not represent all the technical ideas of the present invention. It should be understood that various equivalents and modifications may be substituted therefor at the time of filing this application.
Reference numerals
100,200,300: current collector
110,210,310: metal plate
120,220,320: porous reinforcing material
400: electrode assembly
410: positive current collector
411: positive electrode mixture layer
420: negative current collector
421: negative electrode mixture layer
431: first diaphragm
432: a second diaphragm.

Claims (14)

1. A battery current collector, comprising:
a metal plate in which a plurality of through holes are formed in a thickness direction; and
a porous reinforcing material filled in the through-holes of the metal plate.
2. The current collector of claim 1, wherein the porous reinforcing material comprises at least one selected from the group consisting of a polymeric material, fibers, inorganic particles, and a carbon material.
3. The current collector of claim 1, wherein an area fraction in which the through-holes are formed is in a range of 10% to 90%.
4. A current collector as in claim 1, wherein the porosity of the porous reinforcing material is from 10% to 90% and the air permeability is from 100s/100mL to 4000s/100 mL.
5. A current collector as in claim 1, wherein the porous reinforcement material has an ionic conductivity of 1x10 at 20 ℃-10And more than S/cm.
6. The current collector of claim 1, wherein the porous reinforcing material comprises at least one of Polyethylene (PE), polypropylene (PP), polymethyl methacrylate (PMMA), polyvinylidene fluoride (PVdF), carboxymethyl cellulose (CMC), epoxy, and polyurethane resins.
7. A current collector as in claim 1, wherein the porous reinforcing material has a structure in which fibers having a diameter of 5 to 50 μ ι η and an L/D of 20 or more are dispersed.
8. A current collector as in claim 1, wherein the porous reinforcing material further comprises a lithium salt, and
wherein the lithium salt contains Li as a cation+And comprises a compound selected from the group consisting of F-、Cl-、Br-、I-、NO3 -、N(CN)2 -、BF4 -、ClO4 -、AlO4 -、AlCl4 -、PF6 -、SbF6 -、AsF6 -、BF2C2O4 -、BC4O8 -、(CF3)2PF4 -、(CF3)3PF3 -、(CF3)4PF2 -、(CF3)5PF-、(CF3)6P-、CF3SO3 -、C4F9SO3 -、CF3CF2SO3 -、(CF3SO2)2N-、(FSO2)2N-、CF3CF2(CF3)2CO-、(CF3SO2)2CH-、CF3(CF2)7SO3 -、CF3CO2 -、CH3CO2 -、SCN-And (CF)3CF2SO2)2N-One or more of the group consisting of as an anion.
9. The current collector of claim 1, wherein the porous reinforcement material comprises a type of first inorganic particle selected from the group consisting of BaTiO3、Pb(Zr,Ti)O3(PZT)、Pb1-aLaaZr1-bTibO3(PLZT, wherein 0<a<1，0<b<1)、Pb(Mg1/3Nb2/3)O3-PbTiO3(PMN-PT), hafnium oxide (HfO)2)、SrTiO3、SnO2、CeO2、MgO、NiO、CaO、ZnO、ZrO2、Y2O3、Al2O3、TiO2And SiC.
10. The current collector of claim 1, wherein the porous reinforcement material further comprises at least one type of second inorganic particles selected from the group consisting of lithium phosphate (Li)3PO4) Lithium titanium phosphate (Li)cTid(PO4)3，0<d<2，0<d<3) Lithium aluminum titanium phosphate (Li)aAlbTic(PO4)3，0<a<2，0<b<1，0<c<3)、(LiAlTiP)aOb(0<a<4，0<b<13) Lithium lanthanum titanate (Li)aLabTiO3，0<a<2，0<b<3) Lithium germanium thiophosphate (Li)aGebPcSd，0<a<4，0<b<1，0<c<1，0<d<5) Lithium nitride (Li)aNb，0<a<4，0<b<2)、LiaSibSc(0<a<3，0<b<2，0<c<4) And LiaPbSc(0<a<3，0<b<3，0<c<7) Group (d) of (a).
11. A current collector as in claim 1, wherein the porous reinforcing material comprises a porous polymeric substrate and a porous coating formed on one or both surfaces of the porous polymeric substrate.
12. A secondary battery including an electrode assembly having a structure in which unit cells including a positive electrode, a first separator, and a negative electrode are repeated, and a second separator is located between the unit cells,
wherein at least one of the positive electrode and the negative electrode includes:
a metal plate in which a plurality of through holes are formed in a thickness direction; and
a porous reinforcing material filled in the through-holes of the metal plate.
13. The secondary battery according to claim 12, wherein the positive electrode and the negative electrode each have the following structure: the electrode mixture layer is laminated on one side of the current collector facing the direction of the first separator.
14. The secondary battery according to claim 12, wherein the positive electrode and the negative electrode each have the following structure: an electrode mixture layer is laminated on one surface of the current collector facing in the direction of the first separator, and
wherein the current collector comprises: a metal plate having a plurality of through holes formed in a thickness direction; and a porous reinforcing material filled in the through-holes of the metal plate.
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WO2021075687A1 (en) 2021-04-22

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